Forensic Identification Center, Southwest University of Political Science and Law, Chongqing, 401120, China; Criminal Investigation School, Southwest University of Political Science and Law, Chongqing, 401120, China.
College of Pharmacy, Chongqing Medical University, Chongqing, 400016, China.
Environ Res. 2023 Jun 15;227:115792. doi: 10.1016/j.envres.2023.115792. Epub 2023 Mar 29.
This work designed and synthesized novelly selective, highly efficient and friendly environmental biochar nanomaterial (ZMBC@ChCl-EG) by screening suitable deep eutectic solvent (DES) as the functional monomer via Density Functional Theory (DFT). The prepared ZMBC@ChCl-EG achieved the highly efficient adsorption of methcathinone (MC) and exhibited excellent selectivity as well as good reusability. Selectivity analysis concluded that the distribution coefficient value (K) of ZMBC@ChCl-EG towards MC was 3.247 L/g, which was about 3 times higher than that of ZMBC, corresponding to stronger selective adsorption capacity. The studies of isothermal and kinetics indicated that ZMBC@ChCl-EG had an excellent adsorption capacity towards MC and the adsorption was mainly chemically controlled. In addition, DFT was used to calculate the binding energies between MC and each component. The binding energies were -10.57 kcal/mol for ChCl-EG/MC, -3.15∼-9.51 kcal/mol for BCs/MC, -2.33 kcal/mol for ZIF-8/MC, respectively, suggesting that DES played a major role in enhancing methcathinone adsorption. Lastly, the adsorption mechanisms were revealed by variables experiment combined with characterizations and DFT calculation. The main mechanisms were hydrogen bonding and π-π interaction.
本工作通过密度泛函理论（DFT）筛选合适的深共熔溶剂（DES）作为功能单体，设计并合成了新颖的选择性、高效且环境友好的生物炭纳米材料（ZMBC@ChCl-EG）。所制备的 ZMBC@ChCl-EG 对甲卡西酮（MC）实现了高效吸附，并表现出优异的选择性和良好的可重复使用性。选择性分析得出，ZMBC@ChCl-EG 对 MC 的分配系数（K）值为 3.247 L/g，约为 ZMBC 的 3 倍，表明其对 MC 具有更强的选择性吸附能力。等温线和动力学研究表明，ZMBC@ChCl-EG 对 MC 具有优异的吸附能力，吸附主要受化学控制。此外，还使用 DFT 计算了 MC 与各组分之间的结合能。结合能分别为 ChCl-EG/MC 为-10.57 kcal/mol，BCs/MC 为-3.15∼-9.51 kcal/mol，ZIF-8/MC 为-2.33 kcal/mol，表明 DES 在增强甲卡西酮吸附中起主要作用。最后，通过变量实验结合表征和 DFT 计算揭示了吸附机制。主要机制是氢键和π-π相互作用。
